High-temperature superconductivity emerges from an un-conventional metallic state. This has stimulated strong efforts to understand exactly how Fermi liquids breakdown and evolve into an un-conventional metal. A fundamental question is how Fermi liquid quasiparticle excitations break down in momentum space. Here we show, using angle-resolved photoemission spectroscopy, that the Fermi liquid quasiparticle excitations of the overdoped superconducting cuprate La1.77Sr0.23CuO4 is highly anisotropic in momentum space. The quasiparticle scattering and residue behave differently along the Fermi surface and hence the Kadowaki-Wood's relation is not obeyed. This kind of Fermi liquid breakdown may apply to a wide range of strongly correlated metal systems where spin fluctuations are present.

Photoelectron spectroscopy has been used to study room temperature adsorption of sulfur dioxide on clean and water exposed (0001) surfaces of zinc and zinc oxide. Water has no significant effect either on clean or on SO2 exposed Zn(0001) at the low water pressures used (p < 10− 7 mbar). In the case of the zinc-terminated ZnO(0001) surface, however, water adsorbs dissociatively and OH groups are shown to have a considerable effect on SO2 surface reactions. A strong oxidation reaction occurs between Zn(0001) and SO2 giving various sulfur containing species. On ZnO(0001), SO2 interacts mainly with oxygen sites giving SO3 or SO4 species. It is shown that the ZnO(0001) sample preparation procedure can have large effects on surface chemical and physical properties. Samples cleaned by four different preparation procedures are investigated, namely sputtering only and sputtering followed by annealing at 450 °C, 530 °C and 600–650 °C. Annealing at 600 °C leads to a transition from a partly OH-terminated surface to a triangularly structured surface free from OH groups. Adsorption of SO2 on the latter surface leads to a decreased surface conductivity, which hampers photoemission measurements. Water is shown to block SO2 adsorption sites on both 450 °C and 530 °C annealed samples. On the latter sample, SO2 reduction has been observed to a small extent on the clean surface and to a larger extent when the surface is prehydroxylated. Here, we speculate that water, similar to hydrogen, generates surface zinc clusters on ZnO(0001). Zinc clusters could enable charge transfer to the antibonding LUMO of the SO2 molecule and subsequent dissociation.

Transfer of spectral weight across the magnetic transition in CoO : novel results from high-energy angle-resolved photoelectron spectroscopy

We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-T-c cuprate La1.48Nd0.4Sr0.12CuO4. Data have been acquired at low and high photon energies, h nu=55 and 500 eV, respectively. The two extracted Fermi surfaces show significant differences. The differences can be attributed to either the change in probing depth suggesting dissimilarity of the intrinsic electronic structure between surface and bulk regions, or a considerable c-axis dispersion signaling a strong interlayer coupling. At both photon energies, considerable spectral weight is observed at all points along the Fermi surface and the intensity distribution as well as Fermi-surface shape observed at low as well as high photon energy is markedly different from what has been previously reported for La1.28Nd0.6Sr0.12CuO4 by Zhou [Science 286, 268 (1999)].

Angle-resolved photoemission on underdoped La1.895Sr0.105CuO4 reveals that in the pseudogap phase, the dispersion has two branches located above and below the Fermi level with a minimum at the Fermi momentum. This is characteristic of the Bogoliubov dispersion in the superconducting state. We also observe that the superconducting and pseudogaps have the same d-wave form with the same amplitude. Our observations provide direct evidence for preformed Cooper pairs, implying that the pseudogap phase is a precursor to superconductivity.

An angle-resolved photoemission study of the scattering rate in the superconducting phase of the high-temperature superconductor La2-xSrxCuO4 with x=0.145 and x=0.17, as a function of binding energy and momentum, is presented. We observe that the scattering rate scales linearly with binding energy up to the high-energy scale E-1 similar to 0.4 eV. The scattering rate is found to be strongly anisotropic, with a minimum along the (0,0)-(pi,pi) direction. A possible connection to a quantum-critical point is discussed.

We report an angle-resolved photoemission study of the electronic structure of the pseudogap state in La1.48Nd0.4Sr0.12CuO4 (T-c < 7 K). Two opposite dispersing Fermi arcs are the main result of this study. Several scenarios that can explain this observation are discussed.

We present angle-resolved photoemission spectroscopy data on moderately underdoped La1.855Sr0.145CuO4 at temperatures below and above the superconducting transition temperature. Unlike previous studies of this material, we observe sharp spectral peaks along the entire underlying Fermi surface in the superconducting state. These peaks trace out an energy gap that follows a simple d-wave form, with a maximum superconducting gap of 14 meV. Our results are consistent with a single gap picture for the cuprates. Furthermore our data on the even more underdoped sample La1.895Sr0.105CuO4 also show sharp spectral peaks, even at the antinode, with a maximum superconducting gap of 26 meV.

The charge density in solids is a fundamental parameter. Here we demonstrate that the charge density can be determined by the use of angle resolved photoelectron spectroscopy. The method, which involves a Fourier-like transform from momentum space to real space, is demonstrated by utilizing soft x-ray angle resolved photoelectron spectroscopy to sample the complete three-dimensional Brillouin zone of copper. It is also shown that this can be done in an energy resolved way as to extract the charge density contribution from states of a particular energy.

We present the first study revealing the electronic structure and electron dynamics of the excited adatom state at the Ge(111):Sn(3×3)R30° surface. By the use of time- and angle-resolved photoemission spectroscopy, the normally unoccupied electronic structure of the partly empty Sn adatom can be probed. From the angle-resolved data we conclude that the adatom electrons at the Ge:Sn surface are more delocalized than at the clean Ge(111)c(2×8) surface. A unique pump-and-probe technique, based on a pulsed femtosecond laser-system, has also allowed us to study the recombination process of the excited state. We connect the recombination process of the excited electrons to the coherent fluctuations of the Sn adatoms. As a result we present an estimate for the time between each collective and coherent adatom flip Δt=9ps, i.e. an adatom switching frequency νsw≈0.1THz. We find that our results, contrary to scanning tunneling microscopy measurements [F. Ronci, S. Colonna, S.D. Thorpe, A. Cricenti, G. Le Lay, Phys. Rev. Lett. 95 (2005) 156101], agree very well with values extracted from molecular dynamics simulations found in the literature [J. Avila, A. Mascaraque, E.G. Michel, M.C. Asensio, G. Le Lay, J. Ortega, R. Pérez, F. Flores, Phys. Rev. Lett. 82 (1999) 442; D. Farias, W. Kaminski, J. Lobo, J. Ortega, E. Hulpke, R. Perez, F. Flores, E.G. Michel, Phys. Rev. Lett. 91 (2003) 16103].

We present angle-resolved photoemission data along the M-Gamma-M direction from a Cu2O(111) single crystal, collected at high photon energies (h nu=619 and 891 eV) and T=100 K. Because of the high photon energies and effective background subtraction, our data give a clear picture of the bulk band structure. The results confirm the existence of a hybridized Cu 3d-Cu 4s state located between the two main Cu 3d and O 2p band regions. Several theoretical studies have predicted the existence of this band, but until now it has not been detected in any photoemission measurements. The experimentally derived band structure is compared to local density approximation calculations with and without the Hubbard potential U. The clear band dispersion in our experimental data has enabled us to extract a refined Hubbard U value, which makes it possible to achieve a better agreement between theoretically calculated bands and experimental data.

We have investigated the initial stages of titanyl phthalocyanine (TiOPc) growth on single crystalline ZnO(0 0 0 1). This organic-semiconductor interface is self-organizing as a 2 x 1 pattern appears in a low energy electron diffraction upon deposition of the molecules. To achieve this pattern, the TiOPc is suggested to adsorb standing with the edge of the molecule along the substrate atomic rows. Photoelectron spectroscopy is used to further analyze the interface; a relatively large upwards band bending amounting to 0.5 eV is found and a splitting of the molecules highest occupied molecular orbital occurs after thermal treatment, indicating that the molecules are lying down. (C) 2007 Elsevier B.V. All rights reserved.

An on-board sample cleaver has been developed in order to cleave small and hard-to-cleave samples. To acquire good cleaves from rigid samples the alignment of the cleaving blade with respect to the internal crystallographic planes is crucial. To have the opportunity to mount the sample and align it to the blade ex situ has many advantages. The design presented has allowed us to cleave very tiny and rigid samples, e.g., the high-temperature superconductor La((2-x))Sr(x)CuO(4). Further, in this design the sample and the cleaver will have the same temperature, allowing us to cleave and keep the sample at low temperature. This is a big advantage over prior cleaver systems. As a result, better surfaces and alignments can be realized, which considerably simplifies and improves the experiments.

We present angle-resolved photoelectron spectroscopy data probing the electronic structure of the Nd-substituted high-T_c cuprate La_1.48Nd_0.4Sr_0.12CuO_4 (Nd-LSCO). Data have been acquired at low and high photon energies, hν = 55 and 500 eV, respectively. Earlier comparable low-energy studies of La_1.4-xNd_0.6Sr_xCuO_4 (x = 0.10, 0.12, 0.15) have shown strongly suppressed photoemission intensity, or absence thereof, in large parts of the Brillouin zone. Contrary to these findings we observe spectral weight at all points along the entire Fermi surface contour at low and high photon energies. No signs of strong charge modulations are found. At high photon energy, the Fermi surface shows obvious differences in shape as compared to the low-energy results presented here and in similar studies. The observed difference in shape and the high bulk-sensitivity at this photon energy suggest intrinsic electronic structure differences between the surface and bulk regions.

The existence of coherent quasiparticles near the Fermi energy in the low temperature state of high-temperature superconductors has been well established by angle-resolved photoemission spectroscopy (ARPES). This technique directly probes the momentum-resolved electronic excitation spectrum of the CuO$_2$ planes. We present a study of close to optimally doped La$_{1.83}$Sr$_{0.17}$CuO$_4$ in the superconducting state and report an abrupt change in the quasiparticle spectral function, as we follow the dispersion of the ARPES signal from the Fermi energy up to 0.6 eV. The interruption in the quasiparticle dispersion separates coherent quasiparticle peaks at low energies from broad incoherent excitations at high energies. We find that the boundary between these low-energy and high-energy features exhibits a cosine-shaped momentum dependence, reminiscent of the superconducting d-wave gap. Further intriguing similarities between characteristics of the incoherent excitations and quasiparticle properties (lifetime, Fermi arcs) suggest a close relation between the electronic response at high and low energies in cuprate superconductors.

We have investigated the initial stages of titanyl phthalocyanine (TiOPc) growth on single crystalline ZnO(0001). This organic-semiconductor interface is self-organizing as a 2×1 pattern appears in a low energy electron diffraction upon deposition of the molecules. To achieve this pattern, the TiOPc is suggested to adsorb standing with the edge of the molecule along the substrate atomic rows. Photoelectron spectroscopy is used to further analyze the interface; a relatively large upwards band bending amounting to 0.5eV is found and a splitting of the molecules highest occupied molecular orbital occurs after thermal treatment, indicating that the molecules are lying down.

The work presented in this thesis aims at achieving an increased understanding of the electronic structure of materials whose properties are to a large extent governed by transition metals. All studies are based on data from angle-resolved photoelectron spectroscopy (ARPES) employed on the valence band of the studied systems. In some cases spectroscopic data have also been combined with numerical electronic structure studies performed using a density functional theory computer code. Five of the studies make extensive use of the benefits provided by performing angle-resolved photoelectron spectroscopy at high photon energies. When probed with soft x-ray photons, the near Fermi edge distribution of spectral weight in Nd2-xCexCuO4 and La2-x-yNdySrxCuO4 display significant differences as compared to similar studies performed in the 20-100 eV range of photon energies. This effect can be attributed to the approximate two-fold increase in probing depth as compared to the low photon energy case. However, high photon energies not only give increased probing depth, it also enables a straightforward interpretation of ARPES data from fully three-dimensional compounds in terms of valence band energy dispersion. This principle has been used to study the dispersions in the transition metal oxides CoO and Cu2O as well as in a proof-of-principle study, where copper was used as a test case. CoO exhibits a magnetic phase transition at the Neel temperature, from a paramagnetic state into an antiferromagnetically ordered state. The presented data show a significant shift of spectral weight between different band structure regions as the sample temperature is elevated across the Neel temperature. The Cu2O ARPES data have confirmed the existence of a hybridized Cu 3d - Cu 4s state. Through comparision with theoretically calculated results, a refined value of the Hubbard potential U has been determined. An extensive ARPES dataset from copper, covering the entire Brillouin zone, has in a proof-of-principle study been used to derive the binding-energy resolved valence band charge density. Two ARPES studies of the La2-x-yNdySrxCuO4 system have been performed in the cnventional low photon energy range. The high energy resolution has enabled a detailed study of dispersive features in the near Fermil level region of the valence band.

The work presented in this thesis aims at achieving an increased understanding of the electronic structure of materials whose properties are to a large extent governed by transition metals. All studies are based on data from angle-resolved photoelectron spectroscopy (ARPES) employed on the valence band of the studied systems. In some cases spectroscopic data have also been combined with numerical electronic structure studies performed using a density functional theory computer code. Five of the studies make extensive use of the benefits provided by performing angle-resolved photoelectron spectroscopy at high photon energies. When probed with soft x-ray photons, the near Fermi edge distribution of spectral weight in Nd2-xCexCuO4 and La2-x-yNdySrxCuO4 display significant differences as compared to similar studies performed in the 20-100 eV range of photon energies. This effect can be attributed to the approximate two-fold increase in probing depth as compared to the low photon energy case. However, high photon energies not only give increased probing depth, it also enables a straightforward interpretation of ARPES data from fully three-dimensional compounds in terms of valence band energy dispersion. This principle has been used to study the dispersions in the transition metal oxides CoO and Cu2O as well as in a proof-of-principle study, where copper was used as a test case. CoO exhibits a magnetic phase transition at the Neel temperature, from a paramagnetic state into an antiferromagnetically ordered state. The presented data show a significant shift of spectral weight between different band structure regions as the sample temperature is elevated across the Neel temperature. The Cu2O ARPES data have confirmed the existence of a hybridized Cu 3d - Cu 4s state. Through comparision with theoretically calculated results, a refined value of the Hubbard potential U has been determined. An extensive ARPES dataset from copper, covering the entire Brillouin zone, has in a proof-of-principle study been used to derive the binding-energy resolved valence band charge density. Two ARPES studies of the La2-x-yNdySrxCuO4 system have been performed in the cnventional low photon energy range. The high energy resolution has enabled a detailed study of dispersive features in the near Fermil level region of the valence band.